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Journal of Physics B Atomic and Molecular Physics

Optical collisions and saturated radiative transition rates

Gerard Nienhuis

Published Sep 14, 1981• 23 citations
Publisher

Abstract

The formal structure of the time dependence of the state of an atom in a perturber bath in an intense classical monochromatic radiation field is studied. The authors allow the cross sections of binary collisions to be affected by the radiation field. The result is used to derive an expression for the collision-broadened saturated fluorescence excitation spectrum and absorption rate in terms of a collisional relaxation operator. This operator can be related to the rate of collisionally aided radiative excitation.

DOI
10.1088/0022-3700/14/17/017

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Physical Review A•Nov 1, 1980•0 citations
The formal structure of the time dependence of the state of an atom in a perturber bath in an intense classical monochromatic radiation field is studied. The authors allow the cross sections of binary collisions to be affected by the radiation field. The result is used to derive an expression for the collision-broadened saturated fluorescence excitation spectrum and absorption rate in terms of a collisional relaxation operator. This operator can be related to the rate of collisionally aided radiative excitation.
The authors derive an expression for the spectrum of fluorescence by a two-state atom in a perturber gas irradiated by nearly resonant monochromatic light of arbitrary intensity. The result is fully expressed in terms of the absorption profile that would be measured in a conventional low-intensity absorption experiment and of the rate of radiative and collisional transitions. The present result generalises previous work and the authors demonstrate that expressions obtained before in special cases are recovered by taking the appropriate limits.
The effect of binary collisions on the fluorescence spectrum of an atom in a nearly resonant monochromatic radiation fievd is evaluated in terms of formal relaxation and correlation operators that refer to a single collision. The driving field can be included in the atomic Hamiltonian, and its time dependence is transformed away, giving rise to a modified atom. The authors relate the strengths and the widths of line occurring in the fluorescence spectrum to the rate of optical collisions, and to other elements of the scattering matrix of the modified atom.
A two-state atom in a perturber gas is irradiated by intense light with an arbitrary spectral profile. The authors derive a general expression for the fluorescence spectrum in terms of the conventional low-intensity absorption profile and the spectral density of the incident light. This result, which contains previous results as special limiting cases, describes the transition from the three-line fluorescence spectrum excited by intense monochromatic light and the power-broadened Lorentzian spectrum produced by broad-band excitation.
We have studied the problem of a collisionally perturbed two-level atom in an intense driving field by developing a method which allows us to calculate the field-dependent collision operator in terms of the low intensity field-independent line-broadening function arising in the usual unified theory of pressure broadening. Our relations are exact to all orders in the field in the limiting case of weak collisions, but they are exact also in the complementary case of strong collisions and weak fields. We apply our results to derive explicit expressions for the rate of optical collisions, the fluorescence spectrum in the case of well-separated components, and the absorption during an adiabatic square pulse.
We apply the analysis of paper I to degenerate atomic systems and calculate the effect of correlations between an atom (the absorber) and perturbers in the binary-collision approximation. The result of our calculation is a generalized absorption profile that specifies the final state of the atom an absorption event. This profile is then related to the total intensities of Rayleigh scattering and fluorescence (redistributed radiation) from the atom. The profile is expressed in terms of collision operators that depend on the index of the multipole of the atom that is created. Some of the operators represent correlations between radiative and collisional events and cannot, except in certain limits, be expressed in terms of the usual line-broadening operators. This, of course, implies that one needs extra dynamical information, on top of that obtainable from ordinary absorption experiments, to be able to describe redistribution. Conversely, redistribution offers a probe of collisional dynamics, not given by absorption experiments, via the polarization of fluorescent light. We give practical expressions for the calculation of these operators and discuss their implications.
The effect of correlations between an absorber atom and perturbers in the binary-collision approximation are applied to degenerate atomic systems. A generalized absorption profile which specifies the final state of the atom after an absorption event is related to the total intensities of Rayleigh scattering and fluorescence from the atom. It is suggested that additional dynamical information to that obtainable from ordinary absorption experiments is required in order to describe redistributed atomic radiation. The scattering of monochromatic radiation by a degenerate atom is computed in a binary-collision approximation; an equation of motion is derived for the correlation function which is valid outside the quantum-regression regime. Solutions are given for the weak-field conditions in terms of generalized absorption and emission profiles that depend on the indices of the atomic multipoles.